JOURNAL OF ORGANIC CHEMISTRY
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2019
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IF 4.745
Na Li,Jinku Bai,Xiaolin Zheng,Honghua Rao
An iron-catalyzed methylene forming strategy is disclosed through sequential C–H and C–O bond functionalization of methanol with cosolvent water. This protocol provides an easy and novel access to methylene-tethered imidazo[1,2-a]pyridine and 2-aminopyridine analogues in a sustainable manner and represents a complementary approach to traditional methylene forming strategies.
研究领域:
有机化学
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催化化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jinghu Chen,Mingming Wang,Shude Zhang,Yaju Wang,Jingfeng Hua,Xiangtong Meng,Qineng Xia,Jieshan Qiu,Shaomin Liu
Glycerol hydrogenolysis to 1,3-propanediol (1,3-PDO) is of significance in promoting the biomass valorization. To achieve the efficient conversion, the selective activation of the secondary C–O bonds in the glycerol is vital. In this work, we comparatively investigated the catalytic performances of Pt/Nb 2 W 3 O 14 catalyst for glycerol hydrogenolysis controlled at the reacting conditions of 140 °C and 40 bar. Compared to Pt/WO 3 and Pt/NbO x , the space–time yield (STY) of 1,3-PDO over Pt/Nb 2 W 3 O 14 catalyst can be improved by a factor of 13, reaching 596.4 mg g cat −1 h −1 . The cation ordering of Nb and W on atomic-scale were fully synergized their unique advantages, showing preferential adsorption of the secondary C–O bond under in-situ DRIFTS tracking. The prepared Nb 2 W 3 O 14 is a tetragonal tungsten bronze (TTB) type complex oxides which can effectively promote the dispersion and reduction of Pt nanoparticles. Such strong interaction between Nb 2 W 3 O 14 and Pt can coordinate the precise adsorption and activation of the secondary C–O bond, simultaneously triggering subsequent hydrogenation. Pt/Nb 2 W 3 O 14 affords an ultrahigh activity in glycerol hydrogenolysis to produce 1,3-PDO, tripling the record productivity that was previously reported of these Pt-W based catalysts. This study reported the development of highly synergistic catalyst based on efficient and selective activation of the secondary C–O bond, which can be extended to catalyst design for other biomass valorization.
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2020
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IF 7.888
Yanru Zhu,Jian Zhang,Xiaodan Ma,Zhe An,Shaowei Guo,Xin Shu,Hongyan Song,Xu Xiang,Jing He
Complexity of chemical linkages (C-C/C-H/C-O, C=C/C=O, or C-O-H/C-O-C) in biomass-derived molecules makes the selective activation of targeted bonds much more challenging, expecting well-defined catalysts and definite catalytically-active sites. This work demonstrates an effective gradient reduction strategy to control the definite structure of catalytically-active sites, affording defects-rich nano-twin Cu particles. This strategy just involves the reduction (calcination under H 2 ) of Cu II -containing layered double hydroxides (LDHs) simply with controlling the reduction gradient (interval time) of Cu II species in two chemical micro-environments (Cu II -O-Cu II and Cu II -O-M II/III/IV (M ≠ Cu)) in the brucite-like layer of LDHs. The nano-twin Cu particles efficiently promote the target activation of C-O and C=C in the conversion of furfural to cyclopentanone (CPO). With ~100% furfural conversion, the defects-rich nano-twin Cu particles afford a CPO selectivity of 92%, 50% higher than regular spherical Cu particles. The multi-stepped defect sites, originating from the planar defects, play a decisive role in promoting the CPO selectivity by facilitating the hydro-deoxygenation to C-O of 4-hydroxycyclopentenone (HCP) and hydrogenation to C=C of HCP or cyclopentenone.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Hongyu Qu,Xiangcheng Li,Xiao Han,Junjie Li,Xinqiang Feng,Chuang Liu,Zhendong Wang,Weimin Yang
Rational design of highly efficient non-noble-metal catalysts for the selective hydrogenolysis of biomass platform compounds to produce fuels and fine chemicals is a key pursuit for the sustainable chemical industry. In this work, we report for the first time the synthesis of a Ni-supported germanosilicate zeolite (Ni-SCM-14) catalyst by a simple grinding method, showing both satisfactory yield (90.3%) and good stability in eight cycles for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). Characterization revealed that Ni nanoparticles were highly dispersed on the SCM-14 zeolite with strong interactions. The synergistic effect of highly dispersed Ni hydrogenation sites and the weak acidity activation of the C–O bond provided by SCM-14 is considered to be the key to the efficient hydrogenolysis of HMF. This discovery opens up a new avenue for germanosilicate zeolite to activate the C–O bond.
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
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2025
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IF 4
Jinlin Mei,Zhentao Liu,Zhengkai Cao,Aocheng Wang,Xiaoyang Kong,Aijun Duan,Chunya Wang,Chunming Xu,Xilong Wang
Hierarchical Y/SBA-15 meso-microporous composites (YS- x ) and corresponding highly dispersed catalysts (Ni/YS- x ) were prepared and applied to the production of jet fuel range hydrocarbons by the selective hydrogenation of oleic acid. Small particle size and electron-deficient Ni δ+ are detrimental to the C C bond activation of the η 1 (C)-acyl conformation and inhibit the decarbonylation/decarboxylation pathway. Besides, the activation ability of the C C bond is regulated to avoid excessive cleavage by the acidity and diffusion properties of the hierarchical Ni/YS- x catalysts, thus affecting their hydroisomerization and hydrocracking properties. The abundant acid sites are beneficial to the selective activation of the C O bond of the η 2 (C, O)-aldehyde conformation and the promotion of the reductive deoxygenation pathway. The optimal Ni/YS-1 shows the highest iso / n -alkane ratio ( i / n = 6.26) and superior jet fuel range hydrocarbons yield (48.8%, 340°C), which is a benefit from its outstanding acid–metal balance and worthy diffusion property.
研究领域:
催化
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多孔材料
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化学反应工程
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能量转换
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表面化学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
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2022
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IF 5.436
Zhen Pu,Jianwei Qin,Xiaoguo Fu,Ruizhi Qiu,Bin Su,Maobing Shuai,Fang Li
Fundamental investigation of metal–CO interactions is of great importance for the development of high-performance catalysts to CO activation. Herein, a series of side-on bonded mononuclear lanthanide (Ln) oxocarbonyl complexes OLn(η2-CO) (Ln = La, Ce, Pr, and Nd) have been prepared and identified in solid argon matrices. The complexes exhibit uncommonly low C–O stretching bands near 1630 cm–1, indicating remarkable C–O bond activation in these Ln analogues. The η2-CO ligand in OLn(η2-CO) can be claimed as an anion on the basis of the experimental observations and quantum chemistry investigations, although the CO anion is commonly considered to be unstable with electron auto-detachment. The CO activation in OLn(η2-CO) is attributed to the photoinduced intramolecular charge transfer from LnO to CO rather than the generally accepted metal → CO π back-donation, which conforms to the traditional Dewar–Chatt–Duncanson motif. Energy decomposition analysis combined with natural orbitals for chemical valence calculations demonstrates that the bonding between LnO and η2-CO arises from the combination of dominant ionic forces (>76%) and normal Lewis “acid–base” interactions. The fundamental findings provide guidelines for the catalyst design of CO activation.
研究领域:
无机化学
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物理化学
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chem Catalysis
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2023
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IF 9.4
Rong Wang,Yue Peng,Jane Chung,Zhen Chen,Xiyang Wang,Haibo Yin,Yimin A. Wu,Jingshan Luo,Junhua Li
Summary The electrocatalytic reduction of CO 2 is an attractive method for reducing greenhouse gases and producing chemical feedstocks. However, the activation of C=O bonds limits the reaction kinetics; therefore, understanding the mechanism of C=O bond activation can guide the design of high-performance catalysts. Here, we investigate the C=O bond activation mechanism during the electroreduction of CO 2 to CO on ZnO. Using in situ experimental techniques and quantum chemical calculations , we find that defects in ZnO promote the formation of Zn–ZnO x interfaces during CO 2 reduction, which mediates an intimate-junction exciton state by the metal semiconductor heterophase. This promotes the formation of CO 2 radicals, exposing electron donation centers for CO 2 adsorption and redox centers for cleaving stable C=O bonds. The internal electric field generated by the heterojunction enhances the initial C=O activation by facilitating the interaction between the metalized Zn d-orbital and the O π -orbital in CO 2 .
研究领域:
电化学
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材料科学
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催化
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）